Assessment of air quality for arsenic, cadmium, mercury and nickel in the Netherlands | RIVM

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(1)UHVHDUFKIRU PDQDQGHQYLURQPHQW. RIJKSINSTITUUT VOOR VOLKSGEZONDHEID EN MILIEU NATIONAL INSTITUTE OF PUBLIC HEALTH AND THE ENVIRONMENT. RIVM report 729999 002 $VVHVVPHQWRIDLUTXDOLW\IRUDUVHQLFFDGPLXP PHUFXU\DQGQLFNHOLQWKH1HWKHUODQGV. E.Buijsman December 1999. This investigation has been performed by order and for the account of the Directorate-General for Environmental Protection, Directorate Air & Energy, within the framework of project 729999, ’Scanning- and scouting air measurements’, milestone ’Report’.. RIVM, P.O. Box 1, 3720 BA Bilthoven, telephone: 31 - 30 - 274 91 11; telefax: 31 - 30 - 274 29 71.

(2) RIVM report 729999 002. page 2 of 29. $EVWUDFW The presence of arsenic, cadmium, mercury and nickel in air in the Netherlands has been investigated. Using measurement data, a limited supplemental monitoring effort and the results of modelling calculations, it has been possible to obtain a realistic picture of air quality in the Netherlands with respect to these substances. Background concentrations of arsenic, cadmium and nickel as derived from measurement results range from 0.6-1.1 ng m-3, 0.2-0.4 ng m-3 and 2.0-2.5 ng m-3, respectively. Air quality figures for mercury as derived from model calculations are 2-3 ng m-3. Increased cadmium concentration levels in industrial areas were observed near the Hoogovens (Steelworks) and in the Rijnmond industrial area. Nickel levels increased in the Rijnmond area and were shown to be in good agreement with model calculations. All levels were usually found to be within the air quality objectives. Exceptions here are cadmium and nickel, for which the Negligible Risk levels are locally exceeded in comparing these levels to air quality objectives..

(3) RIVM report 729999 002. page 3 of 29. 6DPHQYDWWLQJ De ondersteuning van de discussie in Europees verband over de invulling van de dochterrichtlijnen van de Europese Kaderrichtlijn Luchtkwaliteit vereist o.a. informatie over de luchtkwaliteit voor arseen, cadmium, kwik en nikkel in Nederland. In dit rapport worden de resultaten van het onderzoek dat is uitgevoerd naar de luchtkwaliteit van deze stoffen, besproken. Een belangrijk aspect van het onderzoek is om potentiële probleemsituaties te inventariseren. Bij het onderzoek is primair gebruik gemaakt van bestaande informatie om de luchtkwaliteit te karakteriseren, Het onderzoek is aangevuld met een beperkte meetinspanning voor die situaties waar op grond van vooronderzoek is gebleken dat de aanwezige kennis te gering is. Deze meetinspanning was gericht op het verbeteren van de kennis over de situatie nabij een aantal brongebieden. De luchtkwaliteit kan getoetst worden aan een aantal luchtkwaliteitdoelstellingen. concentraties in lucht in Nederland worden vooral bepaald door de grootschalige achtergrond, die in de orde van 0,6-1,1 ng m-3 ligt. Er is een gradiënt over Nederland van zuid (‘hoog’) naar noord (‘laag’). In industriegebieden treden nauwelijks verhogingen op. Voor FDGPLXP bedraagt het grootschalig achtergrondniveau in Nederland 0,2 tot 0,4 ng m-3. Ook hier wordt dezelfde gradiënt als voor arseen vastgesteld. Een lokale verhogingen in de orde 100% is vastgesteld nabij de Hoogovens. Een lichte verhoging wordt waargenomen in het Rijnmondgebied. Het achtergrondniveau voor nikkel is in Nederland 2,0-2,5 ng m-3. In het Rijnmondgebied blijken de nikkelconcentraties verhoogd te zijn: 5-15 ng m-3. Deze resultaten komen goed overeen met de resultaten van de modelberekeningen. Uitspraken over de luchtkwaliteit voor NZLN zijn geheel ontleend aan de uitkomsten van modelberekeningen. Het grootschalige achtergrondniveau bedraagt ca. 2-3 ng m-3. Lokale verhogingen zijn op grond van beschikbare emissiegegevens niet te verwachten. Vergelijking met luchtkwaliteitdoelstellingen leert dat de in Nederland voorkomende niveaus veelal onder luchtkwaliteitdoelstellingen liggen. Uitzonderingen zijn cadmium en nikkel waarvoor lokaal de niveaus van het Verwaarloosbaar Risico worden overschreden. $UVHHQ. De natte arseen- en cadmiumdeposities laten geen ruimtelijke afhankelijkheid over Nederland; ze liggen in de orde van 60-240 resp. 80-240 µg m-2 j-1. De natte depositie van kwik bedraagt ca. 20 µg m-2 j-1. De natte depositie van nikkel bedraagt ca. 640 µg m-2 j-1. In het Rijnmondgebied en onmiddellijke omgeving worden verhoogde natte nikkel deposities waargenomen tot ca. 1000 µg m-2 j-1..

(4) RIVM report 729999 002. page 4 of 29. 6XPPDU\ To support the discussion in the European context on the daughter directives of the European Framework Directive on Air Quality will require such data as information on the air quality related to such substances as arsenic, cadmium, mercury and nickel in the Netherlands. This report will discuss the results of the investigation carried out on the quality of the environment when affected by these substances. It is important to inventory the results for potential problem situations. The investigation made primary use of available information to characterise air quality. The research was supplemented with limited monitoring efforts for the situations in which pre-studies had shown the present knowledge to be insufficient. This monitoring effort was focused on improving the knowledge about a situation near a number of source areas. Air quality can be tested for several air quality objectives. concentrations in air in the Netherlands are mostly the result of their large-scale background levels, ranging from 0.6- 1.1 ng m-3 for a gradient across the Netherlands reaching from south (’high’) to north (’low’). Increased concentration levels in industrial areas were practically non-existent. The large-scale background levels for FDGPLXP came to 0.2 to 0.4 ng m-3, where the same gradient as for arsenic was set. An increased local cadmium level in the order of 100% was found near the Hoogovens (Steelworks) and a slight increase observed in the Rijnmond area. The background level for QLFNHO is 2.0-2.5 ng m-3, with increases of 5-15 ng m-3 nickel observed in Rijnmond. These results are in good agreement with model calculations. Air quality figures for PHUFXU\originate exclusively from model calculations, with large-scale background levels representing approximately 2-3 ng m-3. Based on emission data, local increases are not anticipated. These levels are usually found to be within the air quality objectives. Exceptions here are cadmium and nickel, for which the Negligible Risk levels are locally exceeded in comparing these levels to air quality objectives.. $UVHQLF. The wet depositions of arsenic and cadmium acrossthe Netherlands do not allow any spatial dependency; these deposition levels are in the order of 60-240 µg m-2 j-1 and 80-240 µg m-2 j-1, respectively. The wet deposition of mercury comes to ca. 20 µg m-2 j-1. In the Rijnmond area and immediate surroundings, nickel depositions of up to 1000 µg m-1 j-1 have been observed.

(5) RIVM report 729999 002. &RQWHQWV . ,QWURGXFWLRQ. . 0DWHULDODQGPHWKRGV. . . 5HVHDUFKRXWOLQH. . 0RGHOFDOFXODWLRQV. . 0HDVXUHPHQWV. 5HVXOWV. . 0RGHOFDOFXODWLRQV. 3.1.1 3.1.2 3.1.3 3.1.4 3.1.5 3.1.6 . Large-scale background 10 General characteristics of industrial sources 11 Arsenic 11 Cadmium 11 Mercury 11 Nickel 11. 0HDVXUHPHQWV. 3.2.1 3.2.2 3.2.3 3.2.4. Background levels 12 Industrial areas 14 Other situations 15 Precipitation 15. . 'LVFXVVLRQ. . &RQFOXVLRQV. $FNQRZOHGJHPHQWV. 5HIHUHQFHV. $SSHQGL[$. 0DLOLQJOLVW. $SSHQGL[%. 6WDQGDUGGLVSHUVLRQFDOFXODWLRQV. $SSHQGL[&. 6DPSOLQJDQGDQDO\VLVRIPHWDOV. $SSHQGL['. 0HDVXUHPHQWUHVXOWV. page 5 of 29.

(6) RIVM report 729999 002. page 6 of 29. ,QWURGXFWLRQ The ‘Framework Directive on ambient air quality assessment and management’ came into force in 1996 (EU, 1996). Consequential to this general European guideline, a number of daughter directives for specific components would come into force in the course of the next few years. For example, daughter directives have recently been implemented for the substances in the so-called first phase sulphur dioxide, fine particulate and lead (EU, 1999). Proposals of the European Commission for the substances in the second phase, ozone, benzene and carbon monoxide, are under parliamentary discussion. Position papers are in preparation for the remaining substances, or third phase, i.e. polycyclic aromatic hydrocarbons (PAHs), cadmium, arsenic, nickel and mercury, to serve as the basis for EC proposals for the daughter directives. This last group may be facilitated through opinionforming if, for example, sufficient factual information on the presence of these substances in air is available. To meet the last objective cited, the National Institute of Public Health and the Environment (RIVM) carried out a project in 1998/1999 to establish rulings on air quality for PAH, arsenic, cadmium, mercury and nickel; for PAH the focus will be on benzo[a]pyrene. An important aspect will be to inventory situations where raised levels of substances might occur. This report (729999 002) will deal with arsenic, cadmium, mercury and nickel, while in a separate report (729999 001) PAHs are discussed. Chapter 2 of this report will discuss the general set-up, and the methods and materials used in the research, followed by a discussion in Chapter 3 of the results of model calculations and monitoring. Chapter 4 contains the discussion of these results and Chapter 5 the conclusion to the report findings. The more general environmental aspects of arsenic, cadmium, mercury and nickel will not be discussed in this report; please refer to more general publications on arsenic (Slooff HWDO., 1990), cadmium (Ros HWDO., 1988), mercury (Slooff HWDO., 1995) and nickel (Slooff HWDO., 1992)..

(7) RIVM report 729999 002. page 7 of 29. 0DWHULDODQGPHWKRGV 5HVHDUFKRXWOLQH The starting point for this assessment was that use should be made of information already available, especially that derived from measurements. This could possibly be supplemented with the results of model calculations. Dispersion models were supposed to be used to detect potential problem situations near industrial sources. After this, the remaining incompleteness in the information could be examined with a limited monitoring programme. The project plan was formulated and carried out according to this outline. The model instruments will be explained in §2.2, and operational and recent measurement activities will be presented in §2.3. This information has resulted in the definition of limited RIVM monitoring programme, which will be explained at the end of §2.3.. 0RGHOFDOFXODWLRQV The model calculations, with which concentration levels due to industrial sources were estimated, were carried out using the Operational Priority Substances model. Van Jaarsveld (1990; 1995) has described this model. Input data on emission strength, chimney height and heat content for the model were taken from the Dutch Emission Registration. Further details can be found in Appendix B.. 0HDVXUHPHQWV The inventory of operational and recently performed monitoring activities includes: • Measurements of the provincial authority of Limburg for one urban location. These are 24-hour samples, taken every three days. • Measurements of the provincial authority of Noord-Holland near the Hoogovens (Steelworks). These are 24-hour samples, taken every eight days. • Measurements by the provincial authority of Zuid-Holland at a number of regional locations and one industrial location. These are 24-hour samples, taken every six days. • Measurements by RIVM through the Dutch National Air Quality Monitoring Network, taken at three regional and one urban location. These are 24-hour samples, taken every two days. Measurements of these metals found in precipitation are carried out within the Dutch Air Quality Monitoring Network, as well as in some of the regional networks. The results to be reported in this publication came into being in different ways. For this reason measurement results are not directly comparable. Appendix C gives details on sampling and analysis methods..

(8) RIVM report 729999 002. page 8 of 29. The inventory of monitoring activities showed only a limited number of measurements in industrial environments. Furthermore, the model calculations (see further in § 3.1) showed enhanced levels for nickel, and to a lesser extent for cadmium; in two industrial areas. These observations led to the defining of supplemental cadmium and nickel measurements by RIVM on two industrial sites: Beverwijk, near the Hoogovens (Steelworks), and Schiedam in the Rijnmond area. The usual sampling period of 24 hours was chosen. Sampling was done with a PM10 inlet according to the current views on exposure. A characterisation of measurements and monitoring sites of all the institutions/networks is given in Table 1. Figure 1 shows the locations of the sites.. ?. )LJXUH/RFDWLRQVVKRZLQJRSHUDWLRQDORUUHFHQWPHDVXUHPHQWVRIDUVHQLFFDGPLXPPHUFXU\DQGRUQLFNHO. [o regional background ▲ industrial area n urban background. ZHWGHSRVLWLRQ@.

(9) RIVM report 729999 002. page 9 of 29.

(10). 7DEOH0HDVXUHPHQWVRIDUVHQLFFDGPLXPPHUFXU\DQGQLFNHOUHSRUWHGRQKHUH. Location 1). Matrix 3). . Components. Type 2). As, Cd, Ni. Urban background. A. 1/1996-12/1997. Industrial area Industrial area. A A. 1/1998-12/1998 1/1998-12/1998. Regional background Regional background Industrial area Regional background Regional background. A A A A A. 1/1996-12/1998 1/1996-12/1998 1/1998-12/1998 1/1995-12/1998 1/1996-12/1997 As, Cd: 1/1993-12/1998 9/1998-6/1999 As, Cd: 1/1987-12/1998 Ni: 1/1998-5/1999 As, Cd: 1/1987-12/1998 Ni : 1/1998- 5/1999 As, Cd: 1/1993-12/1998 As: 1/1994-12/1997 Cd: 1/1995-12/1998 Hg: 1/1995-12/1998 As, Cd: 1/1993-12/1998 As, Cd: 1/1987-12/1998 Ni: 1/1998-5/1999 Cd: 1/1993-12/1998 As, Ni: 1/1993-12/1997 Cd: 1/1993-12/1998 9/1998-6/1999 As, Cd: 1/1987-12/1998 Ni: 1 /1998-5/1999. Time period. 3URYLQFHRI/LPEXUJ. Maastricht. 3URYLQFHRI1RRUG+ROODQG. IJmuiden Wijk aan Zee. As, Cd, Ni As, Cd, Ni. 3URYLQFHRI=XLG+ROODQG. Bergambacht Hillegom Hoek van Holland Korendijkse Slikken Westland. As, Cd, Ni As, Cd, Ni As, Cd, Ni As, Cd, Ni As, Cd, Ni. 1DWLRQDO,QVWLWXWHRI3XEOLF+HDOWKDQGWKH(QYLURQPHQW 5,90

(11). Beek (133) Beverwijk (555) Biest-Houtakker (230). As, Cd As, Cd, Ni As, Cd, Ni. Regional background Industrial area Regional background. P A A. Bilthoven (627). As, Cd. Regional background. A. De Bilt (628) De Zilk (444). As, Cd As, Cd. Regional background Regional background. P P P. Gilze-Rijen (231) 1) Kollumerwaard (934). As, Cd As, Cd, Ni As, Cd. Regional background Regional background. Rotterdam (434). As, Cd, Ni. Industrial area. P A A P P. Schiedam (439) Vlaardingen (433). As, Cd, Ni As, Cd. Industrial area Urban background/ Industrial area. 1). A A. Not all measurement activities of the networks are shown in this table. RIVM and the provinces of Limburg and Zuid-Holland measure arsenic and cadmium in precipitation at other locations. 2) Type according to network. 3) A: air, P: precipitation..

(12) RIVM report 729999 002. page 10 of 29. 5HVXOWV 0RGHOFDOFXODWLRQV /DUJHVFDOHEDFNJURXQG Results of investigations on the large-scale dispersion pattern of FDGPLXP and QLFNHl are described in Baart HWDO. (1995). The model calculations were, however, carried out with emission data from 1990. For this reason source receptor matrices from this investigation were used to make an update, in other words, the most recent emission data are used to calculate new concentrations for the Netherlands . This has shown that because of the substantial emission reductions in the neighbouring countries (with respect to the Netherlands), the concentrations for cadmium and nickel, and in the Netherlands for cadmium as well, has been considerably reduced, leading in 1990 to a large-scale background level of 0.6 ng m-3 for cadmium and 4.6 ng m-3 for nickel. In 1995 these levels had dropped to 0.3 ng m-3 and 3.6 ng m-3, respectively. The contribution of Dutch sources to the average concentration level in the Netherlands is estimated at 10% for cadmium and 60% for nickel. Results of model calculations for PHUFXU\ at European scale were published by Petersen HWDO. (1995) and Ryaboshapko HWDO. (1998), and for the NW European scale by Baart HWDO. (1995). The European background concentration of ca. 1 ng m-3 mercury in air and 3-5 ng l-1 in rainwater can be derived from these studies. The concentrations calculated for the Netherlands come to ca. 2-3 ng m -3 and 2050 ng l-1, respectively. Mercury, which is supposed to be present as metallic mercury in the atmosphere, is characterised by a relatively long atmospheric residence time and large-scale dispersion pattern. Therefore the calculations also show most of the deposition of mercury in the Netherlands to be caused by foreign sources (see Table 2). 7DEOH2ULJLQRIWKHWRWDOPHUFXU\GHSRVLWLRQ LQ

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(14) . Country of origin. Contribution. Germany The Netherlands 1) Belgium France Great Britain Other anthropogenic sources Natural sources. 35 17 13 6 6 8 15. 1) The total deposition for the whole of the Netherlands is 2338 kg.. No results are available from large-scale dispersion calculations for DUVHQLF.. 1. Emission reductions for FDGPLXP: Belgium (1990-1997) 77%, Germany (1990-1995) 65%. France (19901995) 65%, The Netherlands (1990-1995) 30% Emission reductions for QLFNHl: Belgium (1990-1997) 68%, Germany (1990-1995) 45%, France (1990-1996) 28%, The Netherlands (1990-1995) 4%.

(15) RIVM report 729999 002. page 11 of 29. *HQHUDOFKDUDFWHULVWLFVRILQGXVWULDOVRXUFHV The Emission Registration contains information on emissions, chimney heights and locations of individual (industrial) sources. This allows us to get an impression of the dispersion and load due to individual industrial sources. The following approach has been used: • Sources of emissions are arranged according to the anticipated loads in the surroundings in terms of air concentrations with standard dispersion matrices in relation to a number of chimney height categories; the parameter1 here is the PD[LPXP anticipated concentration. • For ‘high’-score sources, further information is obtained, wherever possible, by permit issuers, usually provincial authorities. In a number of cases the source and the emission circumstances could be better characterised on the basis of this supplementary information. This has usually led to a downward modification of the emission and in this way to a better insight into the necessity of possible monitoring. • Finally, two source areas were selected for supplemental monitoring: one near the Hoogovens complex in Beverwijk and one in Rijnmond.. $UVHQLF Using the OPS model, supplemental dispersion calculations were carried out for Aluminium Delfzijl, which resulted in a maximum anticipated contribution from this source of ca. 10 ng m-3 at a distance of less than 1 km from the source. The increase was on average 0.5 ng m-3 in an area of 5x5 km around the source. At 5 km from the source the contribution decreased by ca. 0.1 ng m-3. In comparison, the Air Quality monitoring station, Kollumerwaard, nearby, measured an arsenic concentration of ca. 0.6 ng m-3 per year.. &DGPLXP The outcomes of the standard dispersion matrices were not reason enough to make supplemental calculations with the OPS model.. 0HUFXU\ The outcomes of the standard dispersion matrices were not reason enough to make supplemental calculations with the OPS model.. 1LFNHO Using the OPS model, supplemental dispersion calculations were carried out for Aluminium Delfzijl, which resulted in a maximum anticipated contribution from this source of ca. 70 ng m-3 at a distance of less than 1 km from the source. The increase was on average 0.3 ng m-3 in an area of 5x5 km around the source. At 5 km from the source the contribution decreased by ca. 0.5 ng m-3. In comparison, the nearby Air Quality monitoring station, Kollumerwaard , measured a nickel concentration of ca. 0.2 ng m-3 per year. Supplemental calculations were also made for the Rijnmond area, characterised by a number of nickel sources, especially in the refineries sector. Using the OPS model, and data on nickel emissions in the Rijnmond area in 1995, a dispersion calculation was carried out. See Figure 2 for the results. The substantial increase above the background levels remained confined to the province of Zuid-Holland. 1 2. See Appendix B for further information. Kollumerwaard is situated ca. 30 km west of Delfzijl..

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(17). 0.001. . 0.000. FRQFHQWUDWLRQRIWRQJP. . 0HDVXUHPHQWV For the sake of clarity a number of situation types will be distinguished: the background, industrial setting and remaining situations.. %DFNJURXQGOHYHOV The background level is described here as the level in situations outside the direct sphere of influence of the Netherlands’ point or surface sources. The regional background level can be derived from the measurement results from the three regional LML locations and a number of locations in ZuidHolland (see Table 3). Arsenic and cadmium background levels have been on the decrease for years, as shown in Figures 3 and 4. Due to a lack of long-range measurement series it is unknown if nickel levels have also been decreasing. An observable gradient showing decreasing concentrations from south to north has been found for arsenic and cadmium, reflecting the influence of the southern source areas of the Netherlands (Figures 5 and 6). For nickel the background levels across the Netherlands are more-or-less uniform. . 7DEOH<HDUO\DYHUDJHV QJP. Station. Biest Houtakker Bilthoven Kollumerwaard Korendijkse Slikken Hillegom Bergambacht.

(18) RIDUVHQLFFDGPLXPDQGQLFNHOLQDLU. Institution/ network1). Arsenic. Cadmium. Nickel. RIVM-LML RIVM-LML RIVM-LML ZH ZH ZH. 1.1 0.85 0.64 0.96 0.94 0.92. 0.39 0.30 0.21 0.52 0.46 0.44. 2.3 2.3 2.1 2.4 4.4 3.3. 1) RIVM-LML : RIVM/National Air Quality Monitoring Network ZH : province of Zuid Holland.

(19) RIVM report 729999 002. page 13 of 29. DUVHQLFFRQFHQWUDWLRQ . QJP ñ. 4 230 [south] 3. 627 [middle] 901/934 [north]. 2 1 0 91. 92. 93. 94. 95. 96. 97. 98. \HDU. )LJXUH'HYHORSPHQWRIDUVHQLFFRQFHQWUDWLRQLQDLU. FDGPLXPFRQFHQWUDWLRQ . QJP ñ. 1 230 [south] 627 [middle] 901/934 [north]. 0 91. 92. 93. 94. 95. 96. 97. 98. \HDU. )LJXUH'HYHORSPHQWRIFDGPLXPFRQFHQWUDWLRQLQDLU. FDGPLXPFRQFHQWUDWLRQ. DUVHQLFFRQFHQWUDWLRQ . . 4. QJP ñ. 1. 3. QJP ñ. 1991. 1991. 1998. 1998. 2 1. 0. 0 230 [south]. 627 [middle]. 901/934 [north]. 230 [zuid]. 901/934 [noord]. ORFDWLRQ. ORFDWLRQ. )LJXUH*UDGLHQWIRUWKHDUVHQLF. 627 [midden]. )LJXUH*UDGLHQWIRUWKHFDGPLXP. FRQFHQWUDWLRQVDFURVVWKH1HWKHUODQGV. FRQFHQWUDWLRQVDFURVVWKH1HWKHUODQGV. DQG. DQG.

(20) RIVM report 729999 002. page 14 of 29. ,QGXVWULDODUHDV In this section results will be presented of measurements with the explicit purpose of establishing the situation in the industrial areas and thus in the immediate vicinity of industrial sources. The two situations concerned here have to do with measurements for two locations: Zuid-Holland and the Rijnmond area, and Noord-Holland, and measurements taken by the province of Noord-Holland near the Hoogovens. In both cases the RIVM carried out monitoring in 1998 and 1999 in Schiedam and Beverwijk, respectively, to supplement the provincial monitoring. These results are summarised in Table 4. The concentrations of arsenic in air in the Netherlands are shown to be determined by the large-scale background level. Arsenic and cadmium levels rise slightly in the Rijnmond area, with increased levels of cadmium near the Hoogovens. Just as discussed in § 3.1.6 there is a clear rise in the nickel level anticipated in the Rijnmond area, as confirmed by the measurement results. . 7DEOH$YHUDJHFRQFHQWUDWLRQOHYHOV QJP.

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(22) . Location. Institution/ network1). Arsenic. Cadmium. Nickel. 1HDUWKH+RRJRYHQV. Beverwijk Wijk aan Zee2). RIVM NH. 0.90 -. 0.57 -. 2.2 -. RIVM RIVM-LML ZH. 1.1 1.23) 0.98. 0.38 0.433) 0.57. 16 4.73) 8.6. 5LMQPRQG. Schiedam Vlaardingen Hoek van Holland 1). RIVM: supplemental measurements for the project ’Scanning and scouting measurements in air’ NH: province of Noord-Holland RIVM-LML: RIVM/National Air Quality Network ZH: province of Zuid-Holland 2) All the measured concentrations are found below the analysis limit of the methods used (5 for arsenic and cadmium; 10 for nickel); reports of average concentrations are therefore of little value (see also Appendix D). 3) Re-calculated concentration to be able to compare the other concentrations measured by RIVM; see also Appendix C.. RIVM has monitored arsenic and cadmium in Vlaardingen since the late 1980s. The development in yearly averages is found in Figure 7. Cadmium concentrations show a consistent decrease, and arsenic has shown a decreasing trend in the last few years.. $UVHQLFDQGFDGPLXPFRQFHQWUDWLRQV . 4. QJP ñ. Arseen 3. Cadmium. 2 1 0 89. 90. 91. 92. 93. 94. \HDU. 95. 96. 97. 98. )LJXUH<HDUO\DYHUDJHIRUDUVHQLF DQGFDGPLXPFRQFHQWUDWLRQVLQDLULQ. .. 9ODDUGLQJHQ.

(23) RIVM report 729999 002. page 15 of 29. 2WKHUVLWXDWLRQV It is unlikely that a local increase in arsenic, cadmium, mercury or nickel will occur outside the direct sphere of influence of individual sources or industrial areas. The measurements taken in Maastricht partly confirm this. The yearly average concentrations (1997) came to 0.7 ng m-3 for arsenic, 0.3 ng m-3 for cadmium and 1.1 ng m-3 for nickel.. 3UHFLSLWDWLRQ in precipitation is measured at a limited number of stations in the National Precipitation Chemistry Monitoring Network (LMRe); these are Rotterdam and the coastal station of Leiduin (replaced later by De Zilk). Up to 1995 the concentrations were almost always found under the analysis limit of the analysis method, i.e. 1.1 µg l-1. Since 1996 a more sensitive method has been applied, resulting in concentrations of ca. 0.1 - 0.3 µg l-1, corresponding to a wet deposition of ca. 80240 µg arsenic m-2 j-1.. $UVHQLF. in precipitation has been measured for years at all the locations of the LMRe. Yearly average concentrations amount to 0.1-0.3 µg l-1, which corresponds to a wet deposition of ca. 80-240 µg cadmium m-2 j-1. In wet deposition there is generally no clear observable gradient.. &DGPLXP. is measured in precipitation at a limited number of stations in the LMRe; these are Rotterdam and the coastal station of Leiduin (replaced later by De Zilk). Up to 1995 the concentrations in De Zilk were almost always found below the analysis limit of the analysis method, i.e. 0.6 µg l-1. Since 1996 a more sensitive method has been applied, resulting in concentrations of ca. 0.8 µg l-1. In Rotterdam the yearly average concentration is ca. 1.2 µg l-1, which means a wet deposition of ca. 1000 µg nickel m-2.. 1LFNHO. In mid-1994 measuring PHUFXU\in precipitationwas started at two stations in the LMRe: De Zilk and De Bilt. Since early 1998 monitoring has only been continued at De Zilk. Yearly average concentrations are in the order of 20-25 ng l-1 mercury per year at both locations. Where the average precipitation is 800 mm this will mean a wet deposition of ca. 20 µg mercury per m2, corresponding well with the outcome of the model calculations (see §3.1.1)..

(24) RIVM report 729999 002. page 16 of 29. 'LVFXVVLRQ The volume of structural measurements for arsenic, cadmium and nickel in the Netherlands is not large. Mercury concentrations in air are not determined at all. Despite this, fairly reliable statements can be made about air quality in relation to these substances. $UVHQLF concentrations are in particular determined by their large-scale background levels, and measurements at regional stations do not give a very good picture of the levels in the Netherlands. The outcomes of the monitoring in the Rijnmond area and near the Hoogovens show hardly any rise when compared with the background levels. The increases in arsenic anticipated near the Hoogovens1, as predicted by the model calculations, could not be confirmed by the measured levels. is measured both at background stations and in a number of industrial areas. This provides good insight into cadmium levels in the Netherlands and into the extent of locally enhanced levels. In the Rijnmond area, the cadmium level is slightly raised, while near the Hoogovens the increase amounts to 100% of the background level; here a local background concentration of 0.3 ng m-3 is assumed; the measured increase near the Hoogovens is, by the way, lower than could be anticipated from the model outcomes2. &DGPLXP. The air quality for QLFNHOcan be characterised by supplemental measurements from RIVM, allowing both the background level and the level of several Dutch source areas to be determined. The model calculations carried out for the sources in the Rijnmond area show a yearly average concentration of 7 to 8 ng m-3. This in good agreement with the local monitoring, which shows concentrations in the order of 5-15 ng m-3. Statements on air quality for PHUFXU\ are completely based on the outcomes of model calculations. The very large-scale dispersion pattern of mercury would probably have limited any extra information from monitoring. The presence of arsenic, cadmium, mercury and nickel in the precipitation in the Netherlands is reasonably to well known. The arsenic and cadmium depositions show no spatial dependence across the Netherlands, although this cannot be said of mercury due to the limited number of monitoring stations. However, on the basis of the large-scale dispersion pattern and the lack of extensive sources of atmospheric mercury, it can be assumed that there would be little variation in the mercury deposition across the Netherlands. Only for nickel has a traditional increase of wet nickel deposition in Rijnmond been established. Just as the increase in nickel concentrations, this raised deposition is confined to the immediate vicinity of the source.. 1 2. The local contribution for the Beverwijk station is estimated at 0.6 ng As m-3 using model calculations. The local contribution for the Beverwijk station is estimated at 0.5 ng Cd m-3 using model calculations..

(25) RIVM report 729999 002. page 17 of 29. &RQFOXVLRQV The presence of arsenic, cadmium, mercury and nickel in air and precipitation has been investigated in the project ’ Scanning and scouting measurements for air’. Measurement data, limited supplemental monitoring efforts and the results of model calculations have made it possible to obtain good insight into air quality in the Netherlands with respect to these substances. The air quality related to these substances can be largely described on the basis of measurement results. Model calculations indicate that problem situations caused by industrial sources practically do not exist. For mercury, the description is largely based on model calculation outcomes. The calculated levels are, however, so low that mercury measurements would probably have not added any information. The air quality for arsenic, cadmium, mercury and nickel in the Netherlands is summarised in Table 5. Comparing these levels with air quality objectives has taught us that the levels present in the Netherlands are usually found below these values1. Exceptions are cadmium and nickel, of which the Negligible Risk (NR) levels are exceeded. . 7DEOH$YHUDJHFRQFHQWUDWLRQVRIDUVHQLFFDGPLXPPHUFXU\DQGQLFNHO QJP

(26) LQDLU. Situation. Arsenic. Cadmium. Mercury. Nickel. Background Rijnmond area Near Hoogovens. 0.6-1.11) 1.0 1.02. 0.2-0.41) 0.4-0.5 0.6. 2-3 -. 2.2 5-15 2.22). 1). Concentration gradient across the Netherlands; the lowest value is in agreement with the situation in the north of the Netherlands, the highest value with the south of the Netherlands. 2) Concentration is approximately comparable to the situational background level.. The presence of arsenic, cadmium, mercury and nickel in precipitation and the resulting deposition is summarised in Table 6. . 7DEOH$YHUDJHFRQFHQWUDWLRQVRIDUVHQLFFDGPLXPPHUFXU\DQGQLFNHO QJP

(27) LQSUHFLSLWDWLRQLQWKH . 1HWKHUODQGV'DWDJLYHQLQJO. Quantity. Concentration Deposition 1) 2). 1. . FRQFHQWUDWLRQ

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(29). GHSRVLWLRQ

(30). . Arsenic. Cadmium. Mercury. Nickel. 0.10-0.30 60-240. 0.10-0.30 80-240. 0.025 20. 0.80 [1.2]2) 640 [1000]2. For the deposition calculation a yearly precipitation of 800 mm was used. The (increased) values in the Rijnmond areas are in parentheses.. $UVHQLF WHO has not established a safe concentration for arsenic. The Netherlands employs an indicative MTR (Maximum Tolerated Risk) value of 500 ng m-3 and a target value of 5 ng m-3. -3 &DGPLXP WHO proposes a guide value of 1-5 ng m ; furthermore, the average concentration may not increase over time. For urban and industrial areas a value of 10-20 ng m-3 is allowed. The Netherlands employs an indicative MTR (Maximum Tolerated Risk) value of 25 ng m-3 and a NR (negligible risk) value of 0.25 ng m-3. -3 0HUFXU\. The Netherlands employs an indicative MTR (Maximum Tolerated Risk) value of 1 ng m and a NR -3 -3 -3 value of 10 ng m ; the limit value employed is 250 ng m and the target value, 2.5 ng m . 1LFNHO WHO has not established a safe concentration for nickel. The Netherlands employs a limit value of 250 ng m-3 and a target value of 2.5 ng m-3..

(31) RIVM report 729999 002. page 18 of 29. $FNQRZOHGJHPHQWV We gratefully acknowledge the experience and expertise offered by the province of Noord-Holland and DCMR (advisory environmental service) Rijnmond in the inception phase of this report, Databases containing the measurements carried out by the provinces of Limburg, Noord-Holland and by DCMR Rijnmond were of value in the reporting phase of the investigation. Measurement data were kindly made available by the above-mentioned institutions. Information on a number of industrial sources was provided by the provinces of Gelderland, Groningen, Limburg and NoordHolland, as well as the Hoogovens. Ruth de Wijs-Christensen is thanked for the editorial assistance..

(32) RIVM report 729999 002. page 19 of 29. 5HIHUHQFHV Baart AC, Berdowski JJM, Jaarsveld JA van. 1995. Calculation of atmospheric deposition of contaminants on the North Sea. Report TNO-MEP-R 95/138. TNO Institute of Environmental Sciences, Energy Research and Process Innovation, Delft, The Netherlands. Elzakker BG van, Buijsman E. 1999. Meetactiviteiten in 1999 in het Landelijk Meetnet Luchtkwaliteit. Report 723101 032. National Institute for Public Health and the Environment, Bilthoven, The Netherlands. EU. 1999. Council Directive 1999/30/EC of 22 April 1999 relating to limit values for sulphur dioxide, nitrogen dioxide and oxides of nitrogen, particulate matter and lead in ambient air. Official Journal of the European Communities. No L 163/41. EU. 1996. Council Directive 96/62/EC of 27 September 1996 on ambient air quality assessment and management. Official Journal of the European Communities. No L 296/55. Jaarsveld JA van. 1990. An operational atmospheric transport model for priority substances; specifications and instructions for use. Report 723301005. National Institute for Public Health and the Environment, Bilthoven ,The Netherlands. Jaarsveld JA van. 1995. Modelling the long-term atmospheric behaviour of pollutants on various spatial scales. Thesis, Utrecht University, the Netherlands. Petersen G, Iverfeldt Å, Munthe H. 1995. Atmospheric mercury species over Central and Northern Europe. Model calculations and comparison with observations from the Nordic Air and Preciptation Network for 1987 and 1998. $WPRVSKHULF(QYLURQPHQW 29, 47-67. Ros JPM, Slooff W (eds.), Apeldoorn ME van, Boer KF de, Canton JH, Gestel CAM van, Heijden CA van der, Heijna-Merkus E, Janus JA, Knaap AGAC, Knoop J, Kranjc EI, Leeuwen FXR van, Loch JPG, Meulen A van der, Minderhoud A, Ros JPM, Wiel HJ van de, Besemer AC, Blokzijl PJ, Feron VJ, Guicherit R, Huldy HJ, Huigen C, Most PFJ van der, Mulder HCM, Schoot-Uiterkamp A, Sinkeldam EJ, Vink GTJ,Vrijer F de. 1988. Integrated Criteria Document Cadmium. Report 758476004. National Institute of Public Health and the Environment, Bilthoven, The Netherlands. Ryaboshapko A, Ilyin I, Gusev A, Afinogenova O. 1998. Mercury in the atmosphere of Europe: concentrations, deposition patterns, transboudary fluxes. Meteorological Synthesizing Centre - East. Moscow. EMEPMC-E Report 7/98. Slooff W, Haring BJA, Hesse JM. 1990. Basisdocument arseen (Integrated criteria document arsenic). Report 758701002. National Institute of Public Health and the Environment, Bilthoven, The Netherlands. Slooff W, Bont PFH, Janus JA, Loos B. 1992. Exploratory report Nickel and nickel compounds. Report 710401017. National Institute of Public Health and the Environment, Bilthoven, The Netherlands. Slooff W, Beelen P van, Annema JA, Janus JA (eds.), Loos B, Boer JLM de, Hesse JM, Iersel AAJ van, Jongbloed RH, Knaap AGAC, Kroese ED, Leeuwen FXR van, Luttik R, Meijer P, Mohn GR, Piersma AH, Vaal MA, Okkerman PC, Dogger JW, Vreeburg KJJ. 1995. Integrated Criteria Document Mercury. Report 601014008. National Institute of Public Health and the Environment, Bilthoven, The Netherlands..

(33) RIVM report 729999 002. $SSHQGL[$. 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28-43 44-70. page 20 of 29. 0DLOLQJOLVW. Directeur Lucht & Eenergie, Ir.A.J.Baayen Ir.T.Blom, Directie Lucht & Energie H.J.M.Hoogland, Hoogovens Staal BV J.Nell, DCMR Milieudienst Rijnmond E.Roekens, Vlaamse Milieumaatschappij, Antwerpen, Begium C.Schoonebeek, Provincie Noord-Holland B.Veldstra, Provincie Limburg Depot van Nederlandse Publikaties en Bibliografie Directie RIVM H.P.Bos Ir.H.S.M.A.Diederen Drs.H.C.Eerens Ir.N.D.van Egmond Ing.B.G.van Elzakker Dr.L.H.J.M.Janssen Ir.F.Langweg Dr.ir.D.van Lith Dr.A.van der Meulen Drs.H.Noordijk Dr.W.A.J.van Pul T.A.Regts Dr.R.Ritsema P.Wolfs Drs.E.Buijsman SBD/Voorlichting & Public Relations Bureau Rapportenregistratie Bibliotheek RIVM Bureau Rapportenbeheer Reserve exemplaren.

(34) RIVM report 729999 002. $SSHQGL[%. page 21 of 29. 6WDQGDUGGLVSHUVLRQFDOFXODWLRQV. Standard dispersion matrices have been used to estimate the maximum concentration due to individual industrial sources. These standard dispersion matrices were calculated with the Operational Priority Substances Model OPS, version 2.1.1, for a limited number of chimney heights (10, 25, 50, 100 m), an emission of 1 g s -1 (≈32 tons a-1) and a heat content of 0 MW. This serves as a quick method to estimate concentration levels from a specific source. Concentrations could then be related to limit values, for example, to see if further research would be necessary. The advantage of this approach is that only a limited number of dispersion calculations have to be carried out. Figure B1 gives an example of a dispersion matrix for a source with a chimney height of 50 m. As the model is linear for the ratio emission/concentration, it is possible to make an easy calculation of the concentration dispersion (and maximum concentration) for each emission strength.. 224 232 240 241 251 244 241 246 270 276 291 316 346 387 390 424 444 458 488 490 485 470 241 246 249 262 260 268 244 247 268 278 288 320 346 416 440 462 492 502 510 525 513 489 259 263 272 269 263 272 263 262 281 314 306 337 384 427 478 514 541 545 548 533 503 482 277 286 283 286 288 281 300 292 300 333 337 367 425 460 524 562 593 602 576 553 533 475 305 300 302 306 295 300 313 322 319 353 351 387 451 502 567 611 640 633 589 570 523 512 329 320 326 314 317 335 343 358 340 355 362 403 490 542 615 663 667 619 603 557 548 527 341 349 343 340 360 362 363 366 379 364 389 413 469 581 658 688 639 594 596 582 559 531 335 368 360 369 390 392 400 391 386 377 411 486 622 763 677 635 601 611 602 580 553 522 344 348 354 350 404 419 425 425 377 344 330 444 622 785 691 575 596 597 581 561 534 508 352 359 360 358 352 342 320 425 357 217 135 778 815 600 665 533 559 596 588 568 539 515 348 358 362 362 359 346 319 256 139 420 848 6941023 515 624 555 583 586 575 559 538 509 339 334 340 342 339 327 297 232 142 240 79114391070 390 530 516 543 549 545 528 506 489 317 326 331 349 429 437 492 487 417 300 458 759 380 556 658 479 505 507 501 488 477 454 347 361 355 369 397 405 390 416 390 308 202 246 313 527 574 565 579 571 471 462 445 428 334 345 348 347 352 355 333 323 308 356 267 320 341 390 493 509 516 514 498 469 416 405 317 328 336 317 310 305 305 265 259 227 259 306 309 345 367 464 466 465 454 421 407 432 293 301 304 288 270 280 250 228 271 236 264 303 298 323 343 359 426 418 388 386 371 394 268 268 272 267 266 253 221 224 250 240 259 290 287 303 319 328 341 362 361 349 370 364 244 243 251 241 237 224 220 239 214 234 251 273 272 282 296 303 309 316 328 351 342 327 223 227 220 217 208 201 219 234 211 227 239 260 279 264 273 281 286 288 330 323 313 304 206 204 199 195 188 192 205 217 210 220 228 246 260 243 256 262 268 254 252 295 287 282 189 189 181 177 177 184 195 183 194 201 220 232 234 229 239 229 232 233 233 230 269 251 grid cell dimensions number of grid points co-ordinates upper left corner average concentration. : 50 m : 22x22 : -525 m, 525 m : 384 ng m-3 . )LJXUH%([DPSOHRIDVWDQGDUGGLVSHUVLRQPDWUL[IRUDVRXUFHZLWKDQHPLVVLRQVWUHQJWKRIJV . DQGDFKLPQH\KHLJKWRIP1XPEHUVUHIHUWR\HDUO\DYHUDJHGFRQFHQWUDWLRQVLQQJP 6RXUFHORFDWLRQLVJLYHQE\0D[LPXPFRQFHQWUDWLRQLVXQGHUOLQHG.

(35) RIVM report 729999 002. page 22 of 29. Tables B1 up to and including B4 give the sources that were first evaluated by standard dispersion matrices and for which it was concluded that high levels could possibly occur. This table also shows first-order estimates for the maximum concentration and the distance D of the maximum. Based on these results, it was concluded that for the Hoogovens (Steelworks) and for the heavily industrialised Rijnmond area, supplementary dispersion calculations on a more spatially detailed level has to be carried out. 7DEOH%)LUVWRUGHUHVWLPDWHVRIPD[LPXPDUVHQLFFRQFHQWUDWLRQV ,QSXWGDWDIURP(PLVVLRQ5HJLVWUDWLRQ. Source. Location. Aluminium Delfzijl Outocompu Hoogovens DSM. Delfzijl Gelderland Beverwijk Geleen. Cmax (ng m-3). D (in m)1). 2000 40 30 20. <100 <100 <100 <100. Remark. See discussion in § 3.1.3 Emission substantially lower2) Supplementary measurements Emission substantially lower 3). 1). The validity of the model does not extend over distances of less than 100 m from the source. Therefore if the model calculates the maximum concentration in the first grid element, ‘<100’ is given as the location of the maximum. 2) Information given by the issuer of the permit, the province of Gelderland. 3) Information given by the issuer of the permit, the province of Limburg. 7DEOH%)LUVWRUGHUHVWLPDWHVRIPD[LPXPFDGPLXPFRQFHQWUDWLRQV ,QSXWGDWDIURP(PLVVLRQ5HJLVWUDWLRQ. Source. Location. Outocompu Budelco Aluminium Delfzijl Hoogovens. Gelderland Budel Delfzijl Beverwijk. Cmax (ng m-3). D (in m)1). 200 100 20 10. <100 <100 <100 <100. Remark. Emission substantially lower2). Supplementary measurements. 1). The validity of the model does not extend over distances of less than 100 m from the source. Therefore if the model calculates the maximum concentration in the first grid element, ‘<100’ is given as the location of the maximum. 2) Information given by the issuer of the permit, the province of Gelderland 7DEOH%)LUVWRUGHUHVWLPDWHVRIPD[LPXPPHUFXU\FRQFHQWUDWLRQV ,QSXWGDWDIURP(PLVVLRQ5HJLVWUDWLRQ. Source. Location. Cmax (ng m-3). D (in m)1). Solvay DSM. Limburg Geleen. 300 200. <100 <100. 1). Remark. The validity of the model does not extend over distances of less than 100 m from the source. Therefore, if the model calculates the maximum concentration in the first grid element, ‘<100’ is given as the location of the maximum..

(36) RIVM report 729999 002. page 23 of 29. 7DEOH%)LUVWRUGHUHVWLPDWHVRIPD[LPXPQLFNHOFRQFHQWUDWLRQV ,QSXWGDWDIURP(PLVVLRQ5HJLVWUDWLRQ. Source. Location. Cmax (ng m-3). D (in m)1). Aluminium Delfzijl Nerefco Bakker Henckels DSM UNI Mills. Delfzijl Pernis Z Holland Overijssel Geleen Z Holland. 1000 1000 700 700 400 400. <100 750 <100 <100 <100 <100. Remark. See discussion in § 3.1.6 Supplementary measurements. 1). The validity of the model does not extend over distances of less than 100 m from the source. Therefore, if the model calculates the maximum concentration in the first grid element, ‘<100’ is given as the location of the maximum.. 0RGHOV. The standard dispersion matrices, for which the results have been presented in Chapter 3, were calculated with the Operational Priority Substances Model, version 2.1.1. Data on emissions, chimney heights and heat content for individual industrial sources are taken from the Emission Registration 1995. Calculations were carried out with long-term averaged meteorological data (1960-1990)..

(37) RIVM report 729999 002. $SSHQGL[&. page 24 of 29. 6DPSOLQJDQGDQDO\VLVRIPHWDOV. 0HDVXUHPHQWV5,90. The sampling of arsenic, cadmium and nickel at the locations of Beverwijk (555) and Schiedam (427) was carried out with the Partisol-Plus 2025 with PM10 inlet, manufactured by Rupprecht & Patashnick. A Teflon filter from Gelman Sciences R2PJ047 was used. Sampling was continuous, with a sampling time of 24 hours. Sampled volume was 24 m3. Biest-Houtakker, Bilthoven, Kollumerwaard and Vlaardingen are locations in the Dutch Air Quality Monitoring Network where metals are re-sampled on a routine basis with medium volume samplers. A Whatman 42 filter is used. Sampling time is 24 hours; total volume is approx. 8 m3. Filters were analysed on a routine basis for arsenic and cadmium, and on this occasion also for nickel. Results obtained with two different sampling methods were used in this research. To facilitate the comparability of the two sampling methods, the standard monitoring network equipment was used at the location of Beverwijk. The Laboratory for Inorganic Analysis at RIVM carried out the analysis. Filters were destructed in a microwave oven with 1.5 M nitric acid for 1½ hours. Analysis was done by ICP-MS. Field and laboratory blanks were taken on a regular basis during the investigation. The results of the measurements carried out in parallel in Beverwijk are shown in Figure C1 to C3. The regression lines shown in these figures can be used to re-calculate the Whatman filter results and thereby make them comparable to the Teflon filter results. This procedure has been used to obtain the results shown in Table 4. $UVHQLF:KDWPDQ. 5. y = 0,716x + 0,0994 2 R = 0,9334. 4. 4. 3. 3. 2. 2. 1. 1. 0 0. 1. 2. 3. 4. 5. 6. 7. $UVHQLF7HIORQ. )LJXUH&&RPSDULVRQRIDUVHQLFFRQFHQWUDWLRQVXVLQJ7HIORQDQG:KDWPDQILOWHUV.

(38) RIVM report 729999 002. page 25 of 29. &DGPLXP:KDWPDQ. 4. y = 0,6639x + 0,0355 2 R = 0,8911. 3. 3. 2. 2. 1. 1. 0 0. 1. 1. 2. 2. 3. 3. 4. 4. 5. 5. &DGPLXP7HIORQ. )LJXUH&&RPSDULVRQRIFDGPLXPFRQFHQWUDWLRQVXVLQJ7HIORQDQG:KDWPDQILOWHUV. 1LNNHO:KDWPDQ. 8. y = 0,4783x + 2,0342 2 R = 0,3682. 7. 6. 5. 4. 3. 2. 1. 0 0. 1. 2. 3. 4. 5. 6. 7. 8. 9. 1LNNHO7HIORQ. )LJXUH&&RPSDULVRQRIQLFNHOFRQFHQWUDWLRQVXVLQJ7HIORQDQG:KDWPDQILOWHUV. 0HDVXUHPHQWV/LPEXUJ. Sampling was carried out with a High Volume Sampler, type GUV-15 H, manufactured by Anderson Samplers Inc./ General Metal Works Inc. The device had an PM-10 size selective sampling inlet, model G 1200. Up to 1994, Whatman 41 type filters made of glass fibre had been used.. Since 1995 QMA filters made of quartz fibre have been used. Sampling took place every 5 days; the sampling period lasted 24 hours.. Filters were analysed in the provinces (Limburg) with ICP..

(39) RIVM report 729999 002. page 26 of 29. 0HDVXUHPHQWV1RRUG+ROODQG. Sampling was carried out with Sierra/Andersen PM10-model 1200-high volume samplers with a PM10 inlet. Whatman QMA quartz fibre filters were used. Sampling period was 24 hours. 0HDVXUHPHQWV=XLG+ROODQG. Sampling was carried out with the Digital DH-80 high volume sampler. Filters from Schleier&Schull, type GF50, and Whatman QM-A type quartz fibre, were used. The flow was approximately 32 m3 h-1. Measurement results were corrected for blanks. Average blank values were calculated using the results of 23 blank filters. Filters were destructed in a microwave oven in a mixture of concentrated nitric acid and hydrochloric acid. Analysis was done with atomic emission spectrometry met ICP-USV. Analysis was continued with ICP-AES according to NEN 6426. A hydride technique was used for arsenic. *HQHUDOUHPDUNVRQVDPSOLQJ. A summary of the most important characteristics of the different sampling methods is given in Table C1. 7DEOH&&KDUDFWHULVWLFVRIWKHVDPSOLQJPHWKRGVE\WKHGLIIHUHQWLQVWLWXWLRQVQHWZRUN. Institution/network. Province of Limburg Province of Noord-Holland Province of Zuid-Holland2) RIVM-LML RIVM3) 1). Flow (m3 h-1). Period. Sampling. Remark. -1) 68 32 0.1 1. 1 day 1 day 1 day 1 day 1 day. Quartz fibre Quartz fibre Quartz fibre Whatman 42 Teflon. PM10 inlet PM10 inlet. PM10 inlet. Information not available. Sampling by DCMR (environmental advice) Rijnmond. 3) Supplementary sampling within the project ‘Scanning and scouting measurements for air’. 2).

(40) RIVM report 729999 002. page 27 of 29. $SSHQGL['. 0HDVXUHPHQWUHVXOWV. 1%7KHPHDVXUHPHQWUHVXOWVLQWKLV$SSHQGL[ZLOOEHSUHVHQWHGDVWKH\ZHUHUHSRUWHGE\WKH LQVWLWXWLRQVQHWZRUNV2QO\EODQNFRUUHFWLRQVZHUHPDGH. . 7DEOH'$UVHQLFFRQFHQWUDWLRQVLQDLU QJP.

(41) DWORFDWLRQVRIWKH'XWFK1DWLRQDO$LU4XDOLW\0RQLWRULQJ. 1HWZRUN. Location. 1991. 1992. 1993. 1994. 1995. 1996. 1997. 1998. 3.0 1.9 1.5 2.5 . .. 2.1 1.4 1.3 1.8 . .. 1.9 1.8 1.3 2.4 . .. 1.6 1.1 1.1 1.2 . .. 1.2 0.99 0.84 0.93 . .. 1.4 1.4 1.1 1.4 . .. 0.98 0.94 0.79 0.99 . .. 1.1 0.85 0.64 0.86 0.901) 1.11). Biest-Houtakker Bilthoven Kollumerwaard Vlaardingen Beverwijk Schiedam. 1). Averaged over the period of September 1998 to June 1999.. . 7DEOH'$UVHQLFFRQFHQWUDWLRQVLQDLU QJP.

(42) DWUHJLRQDOQHWZRUNORFDWLRQV. Location. 1992. 1993. 1994. 1995. 1996. 1997. 1998. . .. . .. . .. . .. . .. . .. . .. <5 <5. . . . . .. . . . . .. . . . . .. . . . . .. . . . . .. 2.0 1.7 1.2 1.9 .. 1.3 1.4 1.4 1.3 .. 0.96 0.94 0.92 . 0.98. .. 1.0. 1.9. 1.5. 1.5. 1.8. 0.7. .. 1991. 3URYLQFHRI1RRUG+ROODQG. De Rijp Wijk aan Zee 3URYLQFHRI=XLG+ROODQG. Korendijkse Slikken Hillegom Bergambacht Westland Hoek van Holland 3URYLQFHRI/LPEXUJ. Maastricht. . 7DEOH'&DGPLXPFRQFHQWUDWLRQVLQDLU QJP.

(43) DWORFDWLRQVRIWKH'XWFK1DWLRQDO$LU4XDOLW\0RQLWRULQJ. 1HWZRUN. Location. 1991. 1992. 1993. 1994. 1995. 1996. 1997. 1998. Biest-Houtakker Bilthoven Kollumerwaard Vlaardingen Beverwijk Schiedam. 0.79 0.56 0.40 0.59 . .. 0.71 0.53 0.35 0.74 . .. 0.63 0.41 0.28 0.62 . .. 0.75 0.51 0.34 0.55 . .. 0.58 0.36 0.20 0.41 . .. 0.42 0.39 0.29 0.42 . .. 0.37 0.39 0.22 0.51 . .. 0.39 0.30 0.21 0.32 0.571) 0.381). 1). Averaged over the period of September 1998 to June 1999..

(44) RIVM report 729999 002. page 28 of 29. . 7DEOH'&DGPLXPFRQFHQWUDWLRQVLQDLU QJP. Location. 1991.

(45) DWORFDWLRQVRIUHJLRQDOQHWZRUNV. 1992. 1993. 1994. 1995. 1996. 1997. 1998. . .. . .. . .. . .. . .. . .. . .. <5 <5. . . . . .. . . . . .. . . . . .. . . . . .. . . . . .. 0.54 0.41 0.34 0.54 .. 0.46 0.33 0.40 0.45 .. 0.52 0.46 0.44 . 0.57. 1.0. 1.0. 1.3. 2.3. 1.1. 0.7. 0.3. .. 3URYLQFHRI1RRUG+ROODQG. De Rijp Wijk aan Zee 3URYLQFHRI=XLG+ROODQG. Korendijkse Slikken Hillegom Bergambacht Westland Hoek van Holland 3URYLQFHRI/LPEXUJ. Maastricht. . 7DEOH'1LFNHOFRQFHQWUDWLRQVLQDLU QJP.

(46) DWORFDWLRQVRIWKH'XWFK1DWLRQDO$LU4XDOLW\0RQLWRULQJ. 1HWZRUN. Location. 1991. 1992. 1993. 1994. 1995. 1996. 1997. 1998. . . . . . .. . . . . . .. . . . . . .. . . . . . .. . . . . . .. . . . . . .. . . . . . .. 2.3 2.3 2.1 4.3 2.21) 161). Biest-Houtakker Bilthoven Kollumerwaard Vlaardingen Beverwijk Schiedam. 1). Averaged over the period September 1998 to June 1999. . 7DEOH'1LFNHOFRQFHQWUDWLRQVLQDLU QJP. Location. 1991.

(47) DWUHJLRQDOQHWZRUNORFDWLRQV. 1992. 1993. 1994. 1995. 1996. 1997. 1998. . .. . .. . .. . .. . .. . .. . .. <10 <10. . . . . .. . . . . .. . . . . .. . . . . .. . . . . .. 5.8 4.7 1.5 . 9.6. 3.0 2.5 2.6 . 8.4. 2.4 4.4 3.3 8.6 .. .. .. .. .. .. .. 1.1. .. 3URYLQFHRI1RRUG+ROODQG. De Rijp Wijk aan Zee 3URYLQFHRI=XLG+ROODQG. Korendijkse Slikken Hillegom Bergambacht Hoek van Holland Westland 3URYLQFHRI/LPEXUJ. Maastricht.

(48) RIVM report 729999 002. page 29 of 29. . 7DEOH'$UVHQLFFRQFHQWUDWLRQVLQSUHFLSLWDWLRQ JO.

(49) DWORFDWLRQVRIWKH'XWFK1DWLRQDO$LU4XDOLW\. 0RQLWRULQJ1HWZRUN. Location. 1993. 1994. 1995. 1996. 1997. 1998. De Zilk Rotterdam. . <1.1. <1.1 <1.1. <1.1 <1.1. 0.30 0.22. 0.07 0.22. . .. . 7DEOH'&DGPLXPFRQFHQWUDWLRQVLQSUHFLSLWDWLRQ JO

(50) DWORFDWLRQVRIWKH'XWFK1DWLRQDO$LU4XDOLW\ 0RQLWRULQJ1HWZRUN. Location. 1993. 1994. 1995. 1996. 1997. 1998. Beek De Bilt De Zilk Gilze-Rijen Kollumerwaard Rotterdam. 0.15 0.13 . 0.13 0.16 0.18. 0.25 0.18 . 0.15 0.12 0.20. 0.30 0.30 0.98 0.12 0.71 0.13. 0.26 0.26 0.13 0.13 0.22 0.19. 0.15 0.12 0.11 0.15 0.24 0.11. . 0.12 0.12 0.08 0.15 0.15. . 7DEOH'1LFNHOFRQFHQWUDWLRQVLQSUHFLSLWDWLRQ JO.

(51) DWORFDWLRQVRIWKH'XWFK1DWLRQDO$LU4XDOLW\. 0RQLWRULQJ1HWZRUN. Location. De Zilk Rotterdam. 1993. 1994. 1995. 1996. 1997. 1998. . 1.5. 0.88 1.1. 0.88 1.2. 0.59 1.2. 0.82 1.2. . .. . 7DEOH'0HUFXU\FRQFHQWUDWLRQVLQSUHFLSLWDWLRQ QJO

(52) DWORFDWLRQVRIWKH'XWFK1DWLRQDO$LU4XDOLW\ 0RQLWRULQJ1HWZRUN. Location. 1993. 1994. 1995. 1996. 1997. 1998. De Bilt De Zilk. . .. . .. 24 25. 28 27. 23 17. . 16.

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